Process for concentrating radioactive combustible waste

ABSTRACT

In the concentration of radioactive combustible waste comprising evaporating and drying a radioactive combustible waste slurry by a thin film drier, the radioactive combustible wastes and an incombustible material, such as sodium sulfate, etc. obtained from a nuclear reactor effluent are mixed together in an amount of not more than 70% by weight, preferably 43 to 70% by weight, of radioactive combustible waste on the basis of a mixture on dry basis, and the mixture is fed to the thin film drier and evaporated and dried therein. A risk of powder explosion and fire is prevented in the drying step thereby.

CROSS REFERENCE TO THE RELATED APPLICATION

This is a continuation-in-part application of patent application Ser. No. 017,825 filed on Mar. 5, 1979.

This invention relates to a process for concentrating a radioactive combustible waste, and more particularly to a process for concentrating a radioactive combustible waste while preventing a risk of powder explosion and fire by the combustible powders.

Various wastes containing radioactive materials are produced by operation of atomic power plants. For example, large amounts of radioactive waste liquor containing inorganic materials such as sodium sulfate, etc., or organic combustible solid wastes such as ion exchange resins, powdery ion exchange resins, filter aids, etc. are produced, and a treatment of such waste liquors and solid wastes is a great problem in operating atomic power plants.

According to one well known method, it is proposed that the radioactive waste liquor is mixed with cement in drums having a capacity of about 200 l, and solidified, and thrown away into oceans, but the number of the drums reserved for such treatment amounts to about 4000 drums per year only for one atomic power plant. Thus, in the case that the radioactive waste is in a solution or in a slurry state containing water, it has been recently proposed to evaporate water from the radioactive waste or further dry and pelletize the waste and solidify the pellets with a hydrophobic solidifying agent such as asphalt, etc. to reduce the volume of the waste, and that it is effective to use a thin film drier for the evaporation (Japanese Laid-open Patent Application Specifications Nos. 64699/75 and 94866/77, and U.S. patent application Ser. No. 846251).

Two processes are available to dry the combustible solid waste produced in the atomic power plant, such as ion exchange resins, powdery ion exchange resins, filter aids, etc. by means of the thin film drier.

One process is to mix ion exchange resins, etc. containing water with hot asphalt in a thin film drier, thereby evaporating the water therefrom and preparing a mixture of dried ion exchange resins, etc. with the asphalt, and to pack the mixture into drums for reservation. The process has a problem such that the water vapor generated within the ion exchange resins, etc. is retained in the ion exchange resins, etc., and the asphalt does not permeate the ion exchange resins, etc., and thus voids remain in the resins when cooled, lowering the strength of the solidified masses of the ion exchange resins, etc. and the asphalt.

Other process is to introduce a slurry of ion exchange resins, etc. into a thin film drier, thereby forming dried powders, and pelletize the powders by a pelletizer. According to the process, the powders are pelletized into pellets for easy handling and also a further advantage such as a large volume reduction can be obtained. The pellets are stable and reservable as such over a long period of time, and can be advantageously applied to any of final cement solidification, asphalt solidification, plastic solidification, etc. as desired. However, the waste powders used as the raw material in said process have very small diameters, for example, about 10 microns, and also the resin powders themselves are combustible and have a fear of fire or powder explosion. For example, a conduit conveying the powders from the thin film drier to the pelletizer is in an air atmosphere, and thus there is a fear of ignition of powders by sparks generated by gears, etc.

An object of the present invention is to provide a process for treating a radioactive combustible waste, which can prevent a fire and powder explosion of the resulting combustible powders when the radioactive combustible waste is dried and concentrated in a thin film drier.

To attain said object, the present invention provides a process for concentrating a radioactive combustible waste by evaporating and drying a slurry of radioactive combustible waste containing combustible wastes in a thin film drier, characterized by mixing the slurry of radioactive combustible waste and an incombustible waste in an amount of not more than 70% by weight of the combustible wastes on the basis of a mixture of the combustible wastes and the incombustible waste on a dry basis, and feeding the resulting mixture to the thin film drier, and evaporating and drying it therein.

The present invention will be described in detail, referring to the accompanying drawings.

FIG. 1 is a partially cut-away view of a thin film drier employed in the present invention.

FIG. 2 is a schematic flow sheet of a process for concentrating a radioactive combustible waste according to one embodiment of the present process.

FIG. 3 is a schematic view of a test apparatus used for determination of an ignition temperature range.

Functional principle of the thin film drier used in the present invention will be described, referring to FIG. 1.

A radioactive waste liquor or slurry is introduced into a thin film drier 1 through a liquid inlet 4 and uniformly distributed onto a heating surface 7 on the vessel wall of the drier by a distributor 5, which comprises a rotating shaft 8 provided at the center of the drier, pivotally movable blades 9 provided on the rotating shaft, and a driving motor 2 for the rotating shaft. Blades 9 are attached to the rotating shaft 8 in positions near the vessel wall, and outwardly extended to and brought in contact with the vessel wall by a centrifugal force developed by the rotation. The waste liquor or slurry vertically flowing down along the heating surface 7 by gravity is formed into a liquid film on the heating surface 7 and heated, evaporated and dried by the heat from a heating jacket 6 at the outside of the vessel wall. A heating medium for the heating jacket 6 is, for example, high pressure steam. The blades 9 scrape off the scales deposited on the heating surface 7 on the vessel wall by rotation. The waste liquor or slurry is concentrated to dried powders, and the resulting powders are taken out of the thin film drier 1 through a powder outlet 10 at the bottom. Vapors generated by the evaporation of the waste liquor or slurry is discharged from a vapor outlet 3 at the upper part of the thin film drier 1 and led to a condenser (not shown in the drawing), where the vapor is condensed to water and reused.

As described above, the blades 9 have two effects, scale removal from the heating surface 7 and promotion of heat exchange at the heating surface 7. Thus, the thin film drier 1 is a compact and highly reliable evaporator.

One embodiment of the present invention will be described in detail below, referring to FIG. 2.

In FIG. 2, granular ion exchange resins produced from a boiling water type reactor as used resins are stored in a slurry state in a used resin tank 11.

The granular ion exchange resins are settled down by gravity in the tank 11 during the storage, and concentrated to a slurry concentration of 60-70% by weight at the bottom of tank 11. Thus, when the used ion exchange resins are transferred to the thin film drier, the content of the tank 11 is stirred to make a uniform slurry, and an immersion pump 18 is provided in the tank 11 to this end.

On the other hand, aqueous solution of sulfuric acid and sodium hydroxide used for regenerating ion exchange resins are mixed and adjusted to a desired pH. The resulting sodium sulfate solution is concentrated in an evaporator (not shown in the drawing) and then stored in a waste liquor tank 12. The amounts of the used resins and the sodium sulfate solution depend upon an operating mode of nuclear reactor and a periodic inspection of the nuclear reactor, and thus widely fluctuate with time. That is, sufficiently large volumes are desirably allocated for the used resin tank 11 and the waste liquor tank 12 to prevent fluctuation with time in the amount of produced wastes to be treated in a waste treatment system of the invention.

The sodium sulfate solution in the waste liquor tank 12 is led to an ejector 13 by a rating pump 17, and mixed with the used resin slurry from the used resin tank 11. The resulting mixture is introduced into a thin film drier 1, and evaporated and dried therein by heat from a heating jacket. Generated vapor is condensed in a condensor 16. Functional principle of evaporation and drying in the thin film drier 1 has been already described, referring to FIG. 1.

The dried powders thus formed are discharged from a powder outlet 10 by gravity, and are pelletized into almond form pellets by a pelletizer 14 and filled in a drum 15. The drum is sealed, when filled up, and then stored in a store house at the atomic power plant site. When a final treatment of plastic solidification or asphalt solidification is selected, the drum is vacuum deaerated, and filled with molten plastic or molten asphalt. The molten plastic or molten asphalt can permeate the pellets owing to the vacuum deaeration to form a rigid solidified mass. When a final treatment of cement solidification is selected, the pellets are dissolved in hot water and mixed with cement.

When mixtures of dried combustible resin powders and dried sodium sulfate powders with various mixing ratios as shown in Table 1 were subjected to ignition tests in the following manner, using a test apparatus shown in FIG. 3 to determine an ignition limit of the mixed powders, it was found that no ignition and combustion took place, if an amount of the combustible resin powders in the mixed powders is not more than 70% by weight on the dry basis.

                  TABLE 1                                                          ______________________________________                                                Ion                 Ratio of                                                   exchange            combustible                                         No.    resin     Na.sub.2 SO.sub.4                                                                        to Na.sub.2 SO.sub.4                                                                   Results                                     ______________________________________                                         1      0.15 g    0.35 g    30%     No ignition                                 2      0.20 g    0.30 g    40%     No ignition                                 3      0.215 g   0.285 g   43%     No ignition                                 4      0.25 g    0.25 g    50%     No ignition                                 5      0.30 g    0.20 g    60%     No ignition                                 6      0.35 g    0.15 g    70%     No ignition                                 7      0.375 g   0.125 g   75%     Ignition                                    8      0.40 g    0.10 g    80%     Ignition                                    ______________________________________                                    

The ignition test was conducted as follows:

Dry ion exchange resin powders (average particle diameter: 10 microns) and dry sodium sulfate powders (average particle diameter: 10 microns) were mixed together in various mixing ratios, and total 0.5 g of said binary mixture was sprayed over a metal net filter 42 in a vessel 41 with an open air vent prepared from a 4-inch steel pipe having a length of 100 mm. Before the spraying, a valve V₁ in a combustion air line 43 was closed, and a valve V₂ was opened, and a valve V₃ was set to a desired air flow rate by adjusting an opening of valve V₃ while reading a flow meter 44. After the spraying of the mixture, valve V₂ was closed, and valve V₁ was opened to supply air into the vessel 41. Then, a spark was generated between wire ends 45 in the vessel 41 by a spark generator and an occurrence of powder explosion was determined by detonation sound.

The combustible wastes produced from a nuclear reactor (granular ion exchange resin, powder ion exchange resin and filter aids) usually amount to 43% by weight or more (on dry basis) of the total weight of combustible wastes and incombustible wastes (as dry powder), and if the combustible wastes are less than 43% by weight (on dry basis), a portion of the combustible wastes remain untreated, and thus a storage tank is required for storing the combustible waste. For example, the smaller the amount of the combustible wastes than 43% by weight (on dry basis), the larger the tank required for their storage. Thus, the mixture of radioactive wastes containing not more than 70% by weight, preferably 43 to 70% by weight of the radioactive combustible wastes (on dry basis) must be treated in the present invention.

One example of drying and pelletizing the following mixed radioactive combustible resins in a mixing proportion of 1:1:1 by weight by a system shown in FIG. 2 is given in Table 2:

                  TABLE 2                                                          ______________________________________                                         Mixed resin characteristics                                                    ______________________________________                                                            Average                                                                        particle Radioactivity                                                         diameter concentration                                      ______________________________________                                         Ion exchange resin (granules)                                                                     200μ  0.6μ Ci/cc                                      Powder resin (powders)                                                                            50μ   0.6μ Ci/cc                                      Filter aid (powders)                                                                              50μ   0.3μ Ci/cc                                      Immersion pump power: 50 kW                                                    ______________________________________                                         Thin film drier operating conditions                                           ______________________________________                                         Heating surface area:    2 m.sup.2                                             Motor output:            3.7 kW                                                Heating steam temperature:                                                                              170° C.                                        Sodium sulfate waste liquor                                                    (sodium sulfate concentration: 20 wt %):                                                                50 kg/hr                                              Mixed resin slurry                                                             (resin concentration: 5 wt %):                                                                          150 kg/hr                                             ______________________________________                                    

The mixed powders obtained by mixing said waste solutions and drying the mixture in the thin film drier under said conditions contained 43% by weight of the combustible resin powders (on dry basis). Pellets could be produced continuously without ignition under the foregoing operating conditions.

The amount of combustible waste such as used resins, etc. discharged from a nuclear reactor is about 60 tons/year and the amount of sodium sulfate in a waste liquor discharged at the same time is about 100 tons/year. When these wastes are mixed together and treated in a thin film drier according to the present invention, an amount of the combustible matters in the mixture is not more than 70% by weight, and thus there is no fear of fire and powder explosion in the drier and successive apparatus. The used resins and the waste liquor can be treated in the thin film drier at the same time, and thus, the treating system is simplified, and the solidified products to be filled in drums are uniform in quality, and thus the storage in the drums and handling of the waste in the final treatment can be advantageously unified.

The present invention can be applied to the treatment of combustible waste and incombustible waste not only from the boiling water type atomic power plant, but also from a pressurized water type atomic power plant, a gas-cooled type atomic power plant, a fast breeder reactor, a reprocessing plant, etc. The incombustible wastes are radioactive inorganic materials obtained from radioactive wastes from nuclear reactor, etc. including, for example, sodium sulfate, sodium nitrate, sodium borate, combustion ashes, etc., and at least one of these radioactive inorganic materials can be used in the present invention as the incombustible waste.

As described above, a fire and powder explosion by combustible powders can be prevented in a thin film drier and successive apparatus in the present invention when the combustible waste is treated, and a radioactive waste disposal can be assured with a good safety thereby. 

What is claimed is:
 1. A process for concentrating radioactive combustible waste comprising:providing a slurry of radioactive combustible waste comprising water and radioactive combustible waste; mixing the slurry of radioactive combustible waste with a slurry of radioactive incombustible waste comprising water and radioactive incombustible waste to form a mixture of radioactive wastes containing 43-70% by weight of radioactive combustible waste as based on a dry mixture of radioactive combustible waste and radioactive incombustible waste; feeding the mixture of radioactive wastes to a thin-film drier; and evaporating the water and drying the mixture of radioactive wastes in the mixture of radioactive wastes therein, thereby concentrating the radioactive combustible waste to powder form.
 2. A process for concentrating radioactive combustible waste comprising:providing a slurry of radioactive combustible waste comprising water and radioactive combustible waste; mixing the slurry of radioactive combustible waste with a slurry of radioactive incombustible waste comprising water and radioactive incombustible waste to form a mixture of radioactive wastes containing 43-70% by weight of radioactive combustible waste as based on a dry mixture of radioactive combustible waste and radioactive incombustible waste; feeding the mixture of radioactive wastes to a thin-film drier with pivotally movable blades; and evaporating the water and drying the mixture of radioactive wastes in the mixture of radioactive wastes therein, thereby concentrating the radioactive combustible waste to dry powder form.
 3. A process for concentrating radioactive combustible waste and preventing spontaneous combustion comprising:providing a slurry of radioactive combustible waste comprising water and radioactive combustible waste; mixing the slurry of radioactive combustible waste with a slurry of radioactive incombustible waste comprising water and radioactive incombustible waste to form a mixture of radioactive wastes containing 43-70% by weight of radioactive combustible waste as based on a dry mixture of radioactive combustible waste and radioactive incombustible waste; feeding the mixture of radioactive wastes to a thin-film drier; and evaporating the water and drying the mixture of radioadtive wastes in the mixture of radioactive wastes therein, thereby concentrating the radioactive combustible waste to powder form.
 4. A process for concentrating radioactive combustible waste and preventing spontaneous combustion comprising:providing a slurry of radioactive combustible waste comprising water and radioactive combustible waste; mixing the slurry of radioactive combustible waste with a slurry of radioactive incombustible waste comprising water and radioactive incombustible waste to form a mixture of radioactive wastes containing 30-70% by weight of radioactive combustible waste as based on a dry mixture of radioactive combustible waste and radioactive incombustible waste; feeding the mixture of radioactive wastes to a thin-film drier; and evaporating the water and drying the mixture of radioactive wastes in the mixture of radioactive wastes therein, thereby concentrating the radioactive combustible waste to powder form.
 5. A process according to claim 1 or 2, wherein the resulting powders are pelletized into pellets.
 6. A process for concentrating radioactive combustible waste comprising:providing a slurry of radioactive combustible waste comprising water and radioactive combustible waste; mixing the slurry of radioactive combustible waste with a slurry of radioactive incombustible waste comprising water and radioactive incombustible waste to form a mixture of radioactive wastes containing 43-70% by weight of radioactive combustible waste as based on a dry mixture of radioactive combustible waste and radioactive incombustible waste; feeding the mixture of radioactive wastes to a thin-film drier with pivotally movable blades; evaporating the water and drying the mixture of radioactive wastes in the mixture of radioactive wastes therein, thereby concentrating the radioactive combustible waste to dry powder form; and pelletizing the dry powder into pellets by a pelletizer.
 7. A process according to claim 1, 2, 6, 3 or 4 wherein the radioactive combustible wastes are organic materials discharged from a nuclear reactor and the incombustible waste is a radioactive incombustible waste.
 8. A process according to claim 7, wherein the organic materials are ion exchange resins, and filter aid.
 9. A process according to claim 7, wherein the radioactive incombustible waste is at least one of sodium sulfate, sodium nitrate, sodium borate and ignition ash, obtained from radioactive wastes from a nuclear reactor. 